The rapid development of high-efficiency and lowprice bifunctional electrocatalysts for replacing precious metal catalysts has been confronted with an enormous challenge for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). Here, a three-dimensional cubic electrocatalyst of nickel− iron complex oxides grown on the rich-nitrogen-doped reduced graphene oxide (NiFe 2 O 4 @N-rGO-CC) was synthesized through the two-step hydrothermal reaction. The experimental integrity test revealed that NiFe 2 O 4 @N-rGO-CC exhibited excellent electrocatalytic performance and long-term stability in both alkaline and acid electrolytes. In a 1.0 M potassium hydroxide (KOH) solution, lower overpotentials of 479 and 156 mV were acquired to deliver the current density of 10 mA•cm −2 for both OER and HER, respectively. Besides, NiFe 2 O 4 @N-rGO-CC also exhibited excellent HER performance in 0.5 M H 2 SO 4 solution, which provided a lower overpotential of 188 mV with a current density of 10 mA•cm −2 . NiFe 2 O 4 @N-rGO-CC showed extremely stable durability over a long time period of 30 h for OER and 50 h for HER in alkaline medium, and 40 h for HER in acid medium. Furthermore, NiFe 2 O 4 @N-rGO-CC required only 1.67 V to deliver the current density of 10 mA•cm −2 for alkaline water splitting, and it could be maintained for up to 70 h without any significant potential reduction. As evidenced, rich N-doped rGO modified the carbon cloth, which could significantly increase the electrocatalytic active sites for OER and HER. This work provided a novel approach for synthesizing transition bimetallic oxides grown on rich N-doped rGO-CC electrocatalysts as an innovative application of the lowcost substitution of precious metal electrocatalysts with highly efficient overall water splitting.